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基于ALD技术的负载型催化剂“自下而上”精细设计
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摘要
实现对催化剂活性位结构的原子级精准调控,是理解催化反应机理和理性设计先进催化剂的基础。原子层沉积(ALD)技术是利用两种前驱体在载体表面上交替发生自饱和、自限制反应的一种薄膜生长技术。由于该技术基于表面自限制反应,因此适合各种不规则表面,包括含有微孔结构的大比表面积催化剂样品。目前利用ALD技术进行新型催化剂制备已经成为人们研究的热点。作为传统湿化学制备催化剂方法的补充,ALD提供了一种随ALD沉积周期"自下而上"近原子级精准构筑催化剂结构的精细技术方法[1,2]。在该报告中,我们将依次讨论ALD制备单原子催化剂[3]、双金属催化剂[4,5]及纳米结构催化剂构筑的成功事例,及其催化性能和反应机理。
Catalyst synthesis with precise control over the structure of catalytic active sites at the atomic level is of essential importance for the scientific understanding of reaction mechanisms and for rational design of advanced catalysts with high performance.Such precise control is achievable using atomic layer deposition(ALD).ALD is similar to chemical vapor deposition(CVD),except that the deposition is split into a sequence of two self-limiting surface reactions between gaseous precursor molecules and a substrate.The unique self-limiting feature of ALD allows conformal deposition of catalytic materials on a high surface area catalyst support at the atomic level.The deposited catalytic materials can be precisely constructed on the support by varying the number and type of ALD cycles.As an alternative to the wet-chemistry based conventional methods,ALD provides a cycle-by-cycle "bottom-up" approach for nanostructuring supported catalysts with near atomic precision.In this presentation,we will discuss synthesis of single-atom catalysts,bimetallic catalysts and nanostructured catalysts using ALD.Their catalytic performance and related reaction mechanism will be as addressed.
引文
[1]Lu,J.L.;Elam,J.W.;Stair,P.C.Surf.Sci.Reps.2016,doi:10.1016/j.surfrep.2016.03.003
    [2]Lu,J.L.;Elam,J.W.;Stair,P.C.Acc.Chem.Res.2013,46:1806
    [3]Yan,H.Cheng,H.;Yi,H.;Lin,Y.;Yao,T.;Wang,C.L.;Li,J.J.;Wei,S.Q.*;and Lu,J.L.,J.Am.Chem.Soc.2015,137:10484-10487.
    [4]Wang,H.W.;Wang,C.L.;Yan,H;Yi,H.;Lu,J.L.,J.Catal.,2015,324:59-68
    [5]Lu,J.L.,et al.,Nat.Commun.,2014,5:3264

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